Synergistic interactions between N3 dye and perovskite CH3NH3PbI3 for aqueous-based photoresponsiveness under visible light

The interactions between molecules and halide perovskite surfaces are important for halide perovskite-based optoelectronic and energy conversion systems. In this manuscript, we investigate the interactions between N3 dye, a famous dye widely employed for dye-sensitized solar cells, and halide perovskite CH 3 NH 3 PbI 3 surface, employing combined experimental and first principles techniques. We find that the interactions between the N3 dye and CH 3 NH 3 PbI 3 are synergistic for the photocurrent generation from the resulting molecule/perovskite photoanode in aqueous solution. The photocurrent values significantly increase by orders of magnitude for the hybrid N3/CH 3 NH 3 PbI 3 system compared with those of the individual components under visible light. The first principles calculations reveal the detailed structural, electronic and optical properties of the N3/CH 3 NH 3 PbI 3 hybrid systems. This study facilitates the fundamental understanding of the interactions between dye molecules and halide perovskite materials, and benefits the design of surface engineered halide perovskite materials for optoelectronic and energy conversion applications.